A new HVE 6 MV AMS system at the University of Cologne

CologneAMS is the new Centre for Accelerator Mass Spectrometry (AMS) at the University of Cologne. It will operate a dedicated AMS system designed to measure all standard cosmogenic nuclides (¹⁰Be,¹⁴C,²⁶Al,³⁶Cl, ⁴¹Ca,¹²⁹I) and which uses a 6 MV Tandetron™ accelerator equipped with an all solid-state power supply, foil and gas stripper. The system also enables a sensitive detection of heavy ions up to ²³⁹U and ²⁴⁴Pu. The high-energy mass-spectrometer consists of a 90 degree magnet with a radius of 2 m and a mass-energy product of 351 AMU MeV to allow the detection of ²⁴⁴Pu⁵⁺ up to the maximum terminal voltage of 6 MV. This magnet is followed by an electrostatic energy analyzer and a switching magnet that can transport the rare isotope beam into various beamlines. The switching magnet forms a third analyzing element which is needed especially for the sensitive detection of heavy elements. So far two beamlines are equipped with their own detection system. One of these lines is used for suppression of isobaric background in the case of the analysis of e.g. ³⁶Cl. This is accomplished by an absorber foil which generates a Z-dependent energy loss in combination with a momentum/charge-state selection via a 120 degree magnet that features up to 30 mrad acceptance for efficient beam transport.In this contribution we will introduce the new Centre, the layout and specific characteristics of the AMS system as well as the main topics of the future scientific work to be performed at CologneAMS.     

Be AMS measurements at low energies (E < 1 MeV)

The longlived isotope ¹⁰Be is of great importance in earth sciences for dating applications, reconstruction of the solar activity or in climate research. Routine AMS measurements with BeO samples are performed on accelerators with a terminal voltage above 2 MV. Applying the degrader foil technique for boron suppression, first tests with BeO samples on the 0.6 MV ETH/PSI machine were limited by background to a ¹⁰Be/⁹Be ratio of 10⁻¹³. The background was identified as ⁹Be which reaches the detector by scattering processes. By applying an additional magnetic mass filter to the high energy mass spectrometer the background was effectively removed. A ¹⁰Be/⁹Be background ratio of <5 × 10⁻¹⁵ was achieved. The overall efficiency (detected ¹⁰Be compared to BeO⁻ injected into the accelerator) was 7-8%.     

10Be and 26Al measurements at the Zurich 6 MV Tandem AMS facility

The setups for the ¹⁰Be and ²⁶Al AMS measurements at the Zurich 6 MV EN Tandem AMS facility are presented and data analysis procedures for both radionuclides are discussed. Performance parameters of the system are shown. In-house AMS standards are compared to commercially available AMS standards.     

Applications of a compact ionization chamber in AMS at energies below 1 MeV/amu

The increasing demand for measuring long-lived radionuclides with small AMS machines at energies below 1 MeV per nucleon raises the need for compact detectors which still have a decent energy resolution and allow for a clear identification of the incident particles. Based on a design by the AMS group at the ETH Zurich a compact gas ionization chamber was built and installed at the 3 MV tandem AMS facility VERA (Vienna Environmental Research Accelerator). The main challenge in AMS is the detection of rare isotope species in the presence of strong isotopic and isobaric interferences. The task of the ionization chamber is the suppression of the unwanted isobar by separating the ions via their different stopping powers. Measurements of ³⁶Cl at VERA showed an achieved suppression of the unwanted stable isobar ³⁶S of 3 × 10⁻⁴ and measurements of ¹⁰Be showed an achieved suppression of ¹⁰B of at least 3 × 10⁻⁶. Additional suppression of the isobaric ions can be achieved by a degrader foil technique applied to ¹⁰Be measurements by G.M. Raisbeck. In combination with the new ionization chamber the achieved suppression of ¹⁰B is at least 10⁻¹⁰. Measurements of blank samples at VERA show that the background for AMS with ¹⁰Be is below 2 × 10⁻¹⁵.     

On the measurement of 10Be on the 1 MV compact AMS system at the Centro Nacional de Aceleradores (Spain)

In this work we present the most recent improvements performed by our group on ¹⁰Be measurements on the 1 MV AMS system recently set up at the CNA (Centro Nacional de Aceleradores), in Seville (Spain). Our efforts have been focused on the study of the viability of our system for BeO and BeF^? measurements. To achieve this, different standard materials have been measured to demonstrate the reliability of the system for BeO measurements in a wide ¹⁰Be/⁹Be atomic ratio range and several environmental samples have been studied both at the 1 MV AMS CNA facility and at the 6 MV AMS ETH-PSI facility of Zurich to validate our measurements. The results show a good agreement between laboratories. New experiments also have been carried out selecting 1+ and 2+ charge states at the exit of the accelerator and inserting Si₃N_3.1 foils with different thicknesses to separate ¹⁰Be from its isobar, ¹⁰B. The influence of each foil on the overall transmission (detected ¹⁰Be compared to BeO^? injected into the accelerator) and background level was also assessed. In addition some tests were also done to assess the viability of BeF₂ and BaBeF₄ measurements at our system. Several metal matrices and cathode preparation procedures for BeO samples were investigated to maximize current and cathode lifetime.     

Carrier-free measurements of natural 10Be/9Be ratios at low energies

At ETH Zurich a new method to measure directly the natural ¹⁰Be/⁹Be ratio of a sample with the compact (0.6 MV) AMS system Tandy has been developed, which allows us to use standard sample preparation methods and AMS techniques. Our results show that carrier-free measurements with compact AMS machines represent a fast, less expensive and more precise alternative for applications where only the relative variation of the ¹⁰Be/⁹Be ratio is needed. Increased source efficiency for (artificial) low carrier samples has been found. If this effect could be exploited for natural samples, it would open the field for other applications like in situ ¹⁰Be-dating of quartz with compact, low energy AMS systems.     

The French accelerator mass spectrometry facility ASTER: Improved performance and developments

Following the installation and acceptance test of the French 5 MV AMS facility ASTER, the focus has been on improving the capability for routine measurements of ¹⁰Be and ²⁶Al. Quality assurance has been established by the introduction of traceable AMS standards for each nuclide, by self-monitoring through participation in round-robin exercises and proficiency testing, and by surveillance of long- and short-time variability of blank and reference materials. A background level of 3 × 10^?14 makes ASTER well-suited for measuring ⁴¹Ca/⁴⁰Ca in the10^?12 region, which is sufficient for a wide range of applications. Routine AMS measurements of volatile elements like ³⁶Cl and ¹²⁹I will most likely become feasible in the very near future as the result of significant improvements in the ion source design.     

Competitive 10Be measurements below 1 MeV with the upgraded ETH–TANDY AMS facility

Competitive ¹⁰Be measurements at energies as low as 0.75 MeV are now possible with the compact ETH AMS system TANDY. In this paper we describe and discuss the modifications that led to the significantly improved performance for ¹⁰Be at the 0.6 MV accelerator. Results from the first routine measurement show that ¹⁰Be on the upgraded TANDY is now fully competitive with larger AMS systems with respect to background and measurement precision. The total efficiency for ¹⁰Be is comparable to our large 6 MV Tandem system and thus sufficient for the full range of applications in the Earth and Environmental Sciences.     

Plutonium measurements on the 1 MV AMS system at the Centro Nacional de Aceleradores (CNA)

Plutonium isotopes have been recently added to the list of radionuclides that can be measured with the new generation of compact AMS facilities. In this paper we present first experimental results concerning the development of the plutonium AMS technique at 680 kV on the 1 MV AMS system at the Centro Nacional de Aceleradores (CNA) in Sevilla, Spain. This is the first compact AMS machine designed and manufactured by High Voltage Engineering Europa. As we demonstrate, the obtained backgrounds for ^239,240Pu, of about 10⁶ atoms, and the ²³⁹Pu/²³⁸U mass suppression factor, in the range of 10⁻⁹, compare to the ones achieved on other AMS facilities. With the measurement of reference materials provided by the International Atomic Energy Agency (IAEA-375, IAEA-Soil-6, IAEA-381) and samples already studied on the 600 kV compact ETH/PSI AMS system at Zürich, we show that the CNA system can be perfectly used for the routine measurement of plutonium isotopes at environmental levels.     

Status of the compact 1 MV AMS facility at the Centro Nacional de Aceleradores (Spain)

Since February 2006, the new 1 MV multielement compact AMS facility SARA (Spanish Accelerator for Radionuclides Analyses) at the Centro Nacional de Aceleradores (CNA) in Sevilla (Spain) is fully operative. During the first one and a half year of operation, the viability of the system for the measurement of ¹⁰Be, ¹⁴C, ¹²⁹I and plutonium isotopes, ²³⁹Pu and ²⁴⁰Pu, has been evaluated. First results have demonstrated that, in terms of precision and detection limits, the performance of the device compares to other compact AMS facilities, although some progress can still be done in order to optimize its capacities. At this moment, background levels are in the order of 10⁻¹⁴ for ¹⁰Be/⁹Be, 10⁻¹³ for ¹²⁹I/¹²⁷I, 10⁻¹⁵ for ¹⁴C/¹²C (processed and unprocessed blank) and about 10⁶ atoms for plutonium isotopes: ²³⁹Pu, ²⁴⁰Pu and ²⁴²Pu. In this work, the current status of the AMS measurements at CNA for the above mentioned radionuclides is described.     

Development of a high intensity Al beam from SiC targets for accelerated beam experiments at ISAC

An intense beam of ^26gAl has been developed for accelerated beam experiments at TRIUMF’s ISAC facility. Studies of the on-line production of Al radionuclides from thick silicon carbide targets have been performed as part of a program of beam development for astrophysical reaction studies at ISAC. While the release of short-lived Al nuclides from SiC was found to be slow, development of new target material forms and high-power target containers has allowed operation of SiC targets with proton currents of up to 70 μA on target. In addition, operation with the TRIUMF resonant ionization laser ion source (TRILIS) has produced ^26gAl beam intensities of 5.1 × 10¹⁰ s⁻¹.     

A new value for the half-life of Be by Heavy-Ion Elastic Recoil Detection and liquid scintillation counting

The importance of ¹⁰Be in different applications of accelerator mass spectrometry (AMS) is well-known. In this context the half-life of ¹⁰Be has a crucial impact, and an accurate and precise determination of the half-life is a prerequisite for many of the applications of ¹⁰Be in cosmic-ray and earth science research. Recently, the value of the ¹⁰Be half-life has been the centre of much debate. In order to overcome uncertainties inherent in previous determinations, we introduced a new method of high accuracy and precision. An aliquot of our highly enriched ¹⁰Be master solution was serially diluted with increasing well-known masses of ⁹Be. We then determined the initial ¹⁰Be concentration by least square fit to the series of measurements of the resultant ¹⁰Be/⁹Be ratio. In order to minimize uncertainties because of mass bias which plague other low-energy mass spectrometric methods, we used for the first time Heavy-Ion Elastic Recoil Detection (HI-ERD) for the determination of the ¹⁰Be/⁹Be isotopic ratios, a technique which does not suffer from difficult to control mass fractionation. The specific activity of the master solution was measured by means of accurate liquid scintillation counting (LSC). The resultant combination of the ¹⁰Be concentration and activity yields a ¹⁰Be half-life of T_1/2 = 1.388 ± 0.018 (1 s, 1.30%) Ma. In a parallel but independent study (Chmeleff et al. [11]), found a value of 1.386 ± 0.016 (1.15%) Ma. Our recommended weighted mean and mean standard error for the new value for ¹⁰Be half-life based on these two independent measurements is 1.387 ± 0.012 (0.87%) Ma.     

AMS measurement technique after 30 years: Possibilities and limitations of low energy systems

A brief summary of the development of AMS over the last 30 years is given and major development steps for the measurement technique are described. With the appearance of compact low energy AMS systems 10 years ago, a new category of AMS instruments has been introduced. This has resulted in a boom of new AMS facilities with more than 20 installations over the last 5 years. But low energy AMS is not limited to radiocarbon only and there is a great potential for ¹⁰Be, ²⁶Al, ¹²⁹I and actinides measurements at compact AMS systems. The latest developments towards the low energy limit of AMS resulted in two new types of systems, the NEC Single Stage AMS and ETH MICADAS operating with terminal voltages of about 200 kV only. These systems have enormous impact, not only on the use of AMS in biomedical research but also on radiocarbon dating. Precision limits of radiocarbon dating will be discussed for the MICADAS type instruments.     

SUERC AMS ion detection

In a short time Be, C, Al, Cl, Ca and I accelerator mass spectrometry (AMS) have been established on the National Electrostatics Corporation (NEC) 5 MV pelletron system at the Scottish Universities Environmental Research Centre (SUERC). While summarising the present performance of the system, this report will focus on the details of ion detection, which sample materials are used and the analytical procedures employed for each individual species during routine analysis.All rare isotope detection is with a single flexible detector and ion event analysis system, but switching of analysed species typically requires a detector reconfiguration. Configurations for routine ¹⁰Be, ¹⁴C, ²⁶Al, ³⁶Cl, ⁴¹Ca and ¹²⁹I detection have been established and will be presented here. Notably, there has proven to be sufficient suppression of the isobaric interferences of ³⁶Cl and ⁴¹Ca in the 5+ charge state using an argon gas stripper at a terminal voltage of 5.0 MV to allow for routine analysis of these isotopes.     

Determination of the Be half-life by multicollector ICP-MS and liquid scintillation counting

A new method was designed and used for determining the half-life of the isotope ¹⁰Be. The method is based on (1) accurate ¹⁰Be/⁹Be measurements of ⁹Be-spiked solutions of a ¹⁰Be-rich master solution using multicollector ICP mass spectrometry (MC-ICP-MS) and (2) liquid scintillation counting (LSC) using the CIEMAT/NIST method for determining the activity concentrations of the solutions whose ¹⁰Be concentrations were determined by mass spectrometry. Important requirements for the success of this approach (a) was the previous coating of glass ampoules filled for counting experiments with ⁹Be, thereby reducing the risk of the adsorptive loss of ¹⁰Be; (b) the removal of Boron from solutions to be measured by MC-ICP-MS by cation chromatography without the introduction of mass fractionation and (c) the accurate determination of the mass bias of ¹⁰Be/⁹Be measurements by ICP-MS which are always affected by the space-charge effect. The mass bias factor was determined to be 1.1862 ± 0.071 for ¹⁰Be/⁹Be from careful fitting and error propagation of ratios of measured Li, B, Si, Cr, Fe, Cu, Sr, Nd, Hf, Tl and U standard solutions of known composition under the same measurement conditions. Employing this factor, an absolute ¹⁰Be/⁹Be ratio of 1.464 ± 0.014 was determined for a first dilution of the ¹⁰Be-rich master solution. This solution is now available as an absolute Be ratio standard in AMS measurements. Finally, a half-life of (1.386 ± 0.016) My (standard uncertainty) was calculated. This value is much more precise than previous estimates and was derived from a fully independent set of experiments. In a parallel, fully independent study using the same master solution, Korschinek et al. [35] have determined a half-life of (1.388 ± 0.018) My. The combined half-life and uncertainty amounts to (1.387 ± 0.012) My. We suggest the use of this value in nuclear studies and in studies that make use of cosmogenic ¹⁰Be in environmental and geologic samples.     

Be radioactive beam production at CIRCE and its utilization in basic and applied physics

A pure ⁷Be beam with an energy E = 1-8 MeV is available for nuclear and applied physics at the 3 MV Pelletron tandem accelerator CIRCE in Caserta. The beam is produced using an offline technique. Typical analyzed beam intensities are about 2 ppA, using cathodes with an activity of the order of 200 MBq. The ⁷Be implantation has been used for both fundamental nuclear physics and applied physics. In particular, different metals have been implanted with ⁷Be in order to study the influence of the chemical composition and of the number of quasi-free electrons of the host material on the ⁷Be half-life. In the field of applied physics, the ⁷Be implantation turns out to be very interesting for wear measurement. In fact, in this case ⁷Be is used as a depth-sensitive tracer. The continuous detection of the sample activity during the wear allows a high sensitivity measurement of wearing speed. The ⁷Be beam production at CIRCE, the implantation procedure and the results obtained from the ⁷Be half-life measurements and the wear characterization of implanted steel samples are described.     

Progress in 14C and 10Be dating at SFU

Since early 1982, a substantial upgrading of the Simon Fraser University radioisotope dating system at the McMaster FN accelerator has taken place. The accelerator itself was equipped with a new charging system and beam tubes, resulting in excellent stability and beam transmission. A new isotope filtering system of two magnets and a Wien filter has removed previously troublesome backgrounds: our carbon background from graphite is now ～ 47 ka BP, and is due to real ¹⁴C rather than scattered ¹³C. Measurement of ¹⁰Be in natural samples is now routine, with several hundred samples processed. Other work on ¹⁰Be has included studies which showed for the first time that ¹⁰Be could be measured at low energies (3 MV). We have also started work on ²⁶Al detection as a preliminary to the investigation of ²⁶Al/¹⁰Be dating. Finally, we present examples of our applications of this facility to studies in oceanography and archaeology.     

High precision C AMS at CIRCE

The CIRCE AMS system started operation in March 2005. The measurement of isotopic ratios ¹⁴C/¹²C in samples of archaeological and environmental interest has rapidly attained high precision and accuracy levels in routine operation. The results of the intercomparison campaign in the framework of the VIRI program, as well as the outcome of a statistical analysis of the about 200 control measurements performed with standard samples, have shown the capability of the whole system for high precision measurements (δR/R < 0.3%), allowing systematic investigations in both archaeological and environmental sciences. ²⁶Al AMS has been implemented for the measurement of the astrophysically relevant ²⁵Mg(p,γ)²⁶Al reaction cross section, while a beam line is under construction for the measurement of actinides isotopic ratios.     

Study of Al measurement on the Shanghai Mini-cyclotron based AMS

We present a modification to the ¹⁴C-dedicated SMCAMS (Shanghai mini-cyclotron based AMS) system to allow the measurement of ²⁶Al for biomedical applications with the existing devices. This is accomplished by determining the turn number, harmonic number and RF frequency theoretically and then making the appropriate orbit programming and beam optics calculation and experimental adjustments. The tests were conducted using pencil graphite (for the carbon pilot beam), Al₂O₃ powder and metal aluminum to accelerate ions with mass number of 24, 25, 26 and 27. The frequency response curves for those ions are shown. Finally, the Al₂O₃ standard sample with a known isotope ratio of 1.0 × 10⁻¹⁰ is measured. The ²⁶Al⁻ ions are detected and its frequency response curve shows the peak of ²⁶Al⁻ though very weak is well separated from the most neighboring interfering molecular ions ²⁵MgH⁻.     

Status and research programs of the multinuclide accelerator mass spectrometry system at the University of Tsukuba

We present the current status and research programs of a multinuclide accelerator mass spectrometry (AMS) system on the 12UD Pelletron tandem accelerator at the University of Tsukuba (Tsukuba AMS system), Japan. A maximum terminal voltage of 12 MV is available for the AMS system. The Tsukuba AMS system can measure environmental levels of long-lived radioisotopes of ¹⁴C, ²⁶Al, ³⁶Cl and ¹²⁹I by employing a molecular pilot beam. Recently, enhancements in AMS techniques and equipment, including sample preparation, the ion source and the data acquisition system, have improved the performance of ³⁶Cl-AMS. The standard deviation of fluctuations is typically ±2%, and the machine background level for the ³⁶Cl/Cl ratio is lower than 1 × 10^?15 with a halite sample. We have measured over 500 samples in 1 year, including samples for earth and environmental sciences and nuclear safety research.